催化作用
选择性
尿素
吸附
氧化物
无机化学
化学工程
化学
材料科学
有机化学
工程类
作者
Danyan Zhang,Yurui Xue,Xuchen Zheng,Chao Zhang,Yuliang Li
摘要
A major impediment to industrial urea synthesis is the lack of catalysts with high selectivity and activity, which inhibits the efficient industrial production of urea. Here, we report a new catalyst system suitable for the highly selective synthesis of industrial urea by in situ growth of graphdiyne on the surface of cobalt-nickel mixed oxides. Such a catalyst is a multi-heterojunction interfacial structure resulting in the obvious incomplete charge-transfer phenomenon between a graphdiyne and metal oxide interface and multiple intermolecular interactions. These intrinsic characteristics are the origin of the high performance of the catalyst. Studies on the mechanism reveal that the catalyst could effectively optimize the adsorption/desorption capacities of the intermediate and promote direct C-N coupling by significantly suppressing by-product reactions toward the formation of H2, CO, N2 and NH3. The catalyst can selectively synthesize urea directly from nitrite and carbon dioxide in water at room temperature and pressure, and exhibits a record-high Faradaic efficiency of 64.3%, nitrogen selectivity (Nurea-selectivity) of 86.0%, carbon selectivity (Curea-selectivity) of ∼100%, as well as urea yield rates of 913.2 μg h-1 mgcat-1 and remarkable long-term stability.
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